Energy-efficient capture of CO2 from power-plant flue gas is one of the grand challenges to reduce greenhouse gas (GHG) emissions. Current CO2-capture technologies are limited by parasitic energy loss, inefficient capture, and unfavorable process economics. We present a novel electrochemical method for CO2 capture from coal-fired power-plant flue gas. The method utilizes in-situ electrochemical pH control with a resin wafer electrodeionization (RW-EDI) device that continuously shifts the pH of the process fluid between basic and acidic in sequential chambers (pH swing). This pH swing enables capture of CO2 from flue gas in the basic chamber followed by release (recovery) of the captured CO2 (purified) in the acidic chamber of the same device. The approach is based on the sensitivity of the thermodynamic equilibrium of CO2 hydration/dehydration reactions over a narrow pH range. The method enables simultaneous absorption (capture) of CO2 from flue gas and desorption (release) at atmospheric pressure without heating, vacuum, or consumptive chemical usage. In other words, the method concentrates CO2 from ∼15% in flue gas to >98% in the recovery stream. To the best of our knowledge, this is the first experimental study focusing on simultaneous capture and release (recovery) of CO2 using an electrochemical method. We describe the method, the role of operating parameters on CO2 recovery, and advancements in process design and engineering for improved efficiency. We report on a method to enhance gas/liquid mixing inside the RW-EDI, which significantly increased CO2 capture rates. We also discuss the importance of using an enzyme/catalyst in enhancing the reaction kinetics. CO2 capture was observed to be a strong function of gas and liquid flow rates and applied electrical field. Up to 80% of the CO2 was captured from a simulated flue gas stream with >98% purity. The results indicate that a narrow pH swing from 8 to 6 (near-neutral pH) could offer a viable pathway for energy-efficient CO2 capture if the reaction kinetics are enhanced. Carbonic anhydrase enzyme enhances the reaction kinetics at near-neutral pH; however, the enzyme lost activity due to the instability at the operating conditions. This observation highlighted the necessity of robust enzymes/catalysts to enhance kinetics of CO2 recovery near-neutral pH.
While bio-oil-derived fuels hold much promise as a replacement for petroleum, transformation of the highly oxygenated mixture has proven challenging. In particular, bio-oils are reactive and difficult to upgrade through catalytic pyrolysis.To reach a stabilized product capable of deep deoxygenation at elevated pressure and temperature, conversion or separation of reactive groups is required. This paper describes an electrochemical process for stabilization and upgrading of bio-oils prior to hydrotreating at high pressure and temperature. This electrolytic process uses a three-compartment cell designed to hydrogenate reactive carbonyl components while separating small acid molecules, such as acetic and formic acids, which act as catalysts for condensation reactions and consume hydrogen gas to produce low-value gases in hydrotreating. To avoid conductivity issues, electrodes are appended to anion-and cation-exchange membranes. The cell was tested using a mixed acetic acid and formic acid surrogate fed to the cathode compartment, where the decrease in the concentration followed the applied charge to the cell. Experiments performed using pine pyrolysis oil demonstrated a significant reduction in the total acid number (TAN), an increase in pH from 2.6 to over 4, and a modest reduction of the carbonyl concentration. Analysis showed the reduction in TAN was primarily due to removal of carboxylic compounds. Experiments observed a decrease in the reactive carbonyl (aldehydes and ketones) concentration that followed applied charge. The results with the newly devised reactor show promise for the electrochemical route for upgrading bio-oils, but significant improvements in TAN removal and carbonyl conversion are needed. Given the distributed nature of biomass, an electrochemical process paired with pyrolysis could be used to densify and stabilize an oil product near the source. The densified liquid could then be shipped to centralized refineries for final upgrading to fuel and/or chemical products.
Membrane capacitive deionization (MCDI) has emerged as an effective and energy efficient desalination technology for treating brackish water streams used in numerous industrial processes. Most material research studies on MCDI focus on improving the porous electrodes or using flowing electrode architectures, and little emphasis is given to the rationale design of ion-exchange membranes (IEMs) for MCDI. In this work, the ionic conductivity, permselectivity, and thickness for three different IEM chemistries (polyaliphatic, poly(arylene ether), and perfluorinated) were correlated to MCDI performance attributes: energy expended per ion removed, salt removal efficiency, and Coulombic efficiency. A 5-to 10-fold reduction in area specific resistance, which accounts for thickness and ionic conductivity, with unconventional perfluorinated and poly(arylene ether) IEMs reduced the energy expended per ion removed in MCDI by a factor of 2 when compared to conventional electrodialysis IEMs. In situ electrochemical impedance spectroscopy substantiated that thinner membranes with higher ionic conductivity helped in the reduction of energy expended per ion removed (more than 50%). Finally, the lower than 100% Coulombic efficiency is ascribed to carbon corrosion of the porous electrodes highlighting that further improvements in MCDI do not just necessitate more appropriate membranes but corrosion resilient electrodes.
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